Improvements in quantum efficiency of excitonic emissions in ZnO epilayers by the elimination of point defects

The internal quantum efficiency $(ηint)$ of the near-band-edge (NBE) excitonic photoluminescence (PL) in ZnO epilayers was significantly improved by eliminating point defects, as well as by the use of ZnO high-temperature-annealed self-buffer layer (HITAB) on a $ScAlMgO4$ substrate as epitaxial templates. Negatively charged Zn vacancy $(VZn)$ concentration was greatly reduced by high-temperature growth, and slower postgrowth cooling (annealing) under minimum oxygen pressure further reduced the gross concentration of positively and negatively charged and neutral point defects, according to the suppression of nonequilibrium defect quenching. The nonradiative PL lifetime $(τnr)$ at room temperature was increased by decreasing the gross concentration of point defects, as well as by decreasing the concentration of $VZn$⁠. Accordingly, certain point defect complexes incorporated with $VZn$ (⁠$VZn-X$ complexes) are assigned to the dominant nonradiative recombination centers. As a result of the elimination of point defects, a record long $τnr$ $(3.8ns)$ at $300K$ was demonstrated. Because the radiative lifetime $(τr)$ is in principle constant in bulk and epitaxial ZnO, the increase in $τnr$ gave rise to the increase in $ηint$⁠. Rich structures originating from exciton-polaritons and excited states of excitons were eventually observed in the low-temperature PL spectrum of the improved ZnO epilayer on HITAB, of which $ηint$ of the NBE emission was 6.3% at $300K$⁠.